Abstract

The third- and fifth-order time-domain Raman responses of liquid carbon disulfide have been calculated, taking local field effects into account through the dipole-induced dipole approximation to the polarizability. The third-order response is shown to be in excellent agreement with experimental data. The calculated two-dimensional shape of the fifth-order response is compared with recently reported experimental observations of what is claimed to be pure fifth-order response. Considerable discrepancies are observed which might be explained by contamination of the experimental results with sequential and especially parallel third-order cascaded Raman response. A new choice of polarization conditions is proposed, which increases the discrimination against these unwanted cascading effects, as compared to the previously discussed fully polarized and magic angle conditions.